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Register a new userThe magnetic ground state of Sr2IrO4 and implications for second-harmonic generation
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The currently accepted magnetic ground state of Sr2IrO4 (the -++- state) preserves inversion symmetry. This is at odds, though, with recent experiments that indicate a magnetoelectric ground state, leading to the speculation that orbital currents or more exotic magnetic multipoles might exist in this material. Here, we analyze various magnetic configurations and demonstrate that two of them, the magnetoelectric -+-+ state and the non-magnetoelectric ++++ state, can explain these recent second-harmonic generation (SHG) experiments, obviating the need to invoke orbital currents. The SHG-probed magnetic order parameter has the symmetry of a parity-breaking multipole in the -+-+ state and of a parity-preserving multipole in the ++++ state. We speculate that either might have been created by the laser pump used in the experiments. An alternative is that the observed magnetic SHG signal is a surface effect. We suggest experiments that could be performed to test these various possibilities, and also address the important issue of the suppression of the RXS intensity at the L2 edge.
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Sr$_2$CuO$_2$Cl$_2$ (SCOC) is a model undoped cuprate with $I4/mmm$ crystallographic symmetry, and a simple magnetic space group $C_Amca$ with associated magnetic point group $mmm1$. However, recent second harmonic spectroscopy in the antiferromagnetic phase has challenged this picture, suggesting instead a magnetic point group $4/mmm$ that co-exists with the antiferromagnetism and breaks the two orthogonal mirror planes containing the tetragonal $c$-axis. Here, we analyze the symmetry of SCOC in light of the second harmonic results, and discuss possible ground states that are consistent with the data.
An anomalous optical second-harmonic generation (SHG) signal was previously reported in Sr$_2$IrO$_4$ and attributed to a hidden odd-parity bulk magnetic state. Here we investigate the origin of this SHG signal using a combination of bulk magnetic susceptibility, magnetic-field-dependent SHG rotational anisotropy, and overlapping wide-field SHG imaging and atomic force microscopy measurements. We find that the anomalous SHG signal exhibits a two-fold rotational symmetry as a function of in-plane magnetic field orientation that is associated with a crystallographic distortion. We also show a change in SHG signal across step edges that tracks the bulk antiferromagnetic stacking pattern. While we do not rule out the existence of hidden order in Sr$_2$IrO$_4$, our results altogether show that the anomalous SHG signal in parent Sr$_2$IrO$_4$ originates instead from a surface-magnetization-induced electric-dipole process that is enhanced by strong spin-orbit coupling.
We investigate the structural and magnetic origins of the unusual ultrafast second-harmonicgeneration (SHG) response of femtosecond-laser-excited nickel oxide (NiO) previously attributed to oscillatory reorientation dynamics of the magnetic structure induced by d-d excitations. Using time-resolved x-ray diffraction from the (3/2 3/2 3/2) magnetic planes, we show that changes in the magnitude of the magnetic structure factor following ultrafast optical excitation are limited to $Delta<F_m>/<F_m>$ = 1.5% in the first 30 ps. An extended investigation of the ultrafast SHG response reveals a strong dependence on wavelength as well as characteristic echoes, both of which give evidence for an acoustic origin of the dynamics. We therefore propose an alternative mechanism for the SHG response based on perturbations of the nonlinear susceptibility via optically induced strain in a spatially confined medium. In this model, the two observed oscillation periods can be understood as the times required for an acoustic strain wave to traverse one coherence length of the SHG process in either the collinear or anti-collinear geometries.
Strong second-harmonic generation has recently been experimentally observed from metamaterials consisting of periodic arrays of metal split ring resonators with an effective negative magnetic permeability [Science, 313, 502 (2006)]. To explore the underlying physical mechanism, a classical model derived from microscopic theory is employed here. The quasi-free electrons inside the metal are approximated as a classical Coulomb-interacting electron gas, and their motion under the excitation of an external electromagnetic field is described by the cold-plasma wave equations. Through numerical simulations, it is demonstrated that the microscopic theory includes the dominant physical mechanisms bothqualitatively and quantitatively.
The ground state electronic structure and magnetic behaviors of curium dioxide (CmO$_{2}$) are controversial. In general, the formal valence of Cm ions in CmO$_{2}$ should be tetravalent. It implies a $5f^{6.0}$ electronic configuration and a non-magnetic ground state. However, it is in sharp contrast with the large magnetic moment measured by painstaking experiments. In order to clarify this contradiction, we tried to study the ground state electronic structure of CmO$_{2}$ by means of a combination of density functional theory and dynamical mean-field theory. We find that CmO$_{2}$ is a wide-gap charge transfer insulator with strong 5$f$ valence state fluctuation. It belongs to a mixed-valence compound indeed. The predominant electronic configurations for Cm ions are $5f^{6.0}$ and $5f^{7.0}$. The resulting magnetic moment agrees quite well with the experimental value. Therefore, the magnetic puzzle in CmO$_{2}$ can be appropriately explained by the mixed-valence scenario.
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